dorsal/arxiv
View SchemaImportance of electronic self-consistency in the TDDFT based treatment of nonadiabatic molecular dynamics
| Authors | T. A. Niehaus, D. Heringer, B. Torralva, Th. Frauenheim |
|---|---|
| Categories | |
| ArXiv ID | physics/0411104 |
| URL | https://arxiv.org/abs/physics/0411104 |
| DOI | 10.1140/epjd/e2005-00079-7 |
Abstract
A mixed quantum-classical approach to simulate the coupled dynamics of electrons and nuclei in nanoscale molecular systems is presented. The method relies on a second order expansion of the Lagrangian in time-dependent density functional theory (TDDFT) around a suitable reference density. We show that the inclusion of the second order term renders the method a self-consistent scheme and improves the calculated optical spectra of molecules by a proper treatment of the coupled response. In the application to ion-fullerene collisions, the inclusion of self-consistency is found to be crucial for a correct description of the charge transfer between projectile and target. For a model of the photoreceptor in retinal proteins, nonadiabatic molecular dynamics simulations are performed and reveal problems of TDDFT in the prediction of intra-molecular charge transfer excitations.
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"abstract": "A mixed quantum-classical approach to simulate the coupled dynamics of\nelectrons and nuclei in nanoscale molecular systems is presented. The method\nrelies on a second order expansion of the Lagrangian in time-dependent density\nfunctional theory (TDDFT) around a suitable reference density. We show that the\ninclusion of the second order term renders the method a self-consistent scheme\nand improves the calculated optical spectra of molecules by a proper treatment\nof the coupled response. In the application to ion-fullerene collisions, the\ninclusion of self-consistency is found to be crucial for a correct description\nof the charge transfer between projectile and target. For a model of the\nphotoreceptor in retinal proteins, nonadiabatic molecular dynamics simulations\nare performed and reveal problems of TDDFT in the prediction of intra-molecular\ncharge transfer excitations.",
"arxiv_id": "physics/0411104",
"authors": [
"T. A. Niehaus",
"D. Heringer",
"B. Torralva",
"Th. Frauenheim"
],
"categories": [
"physics.chem-ph",
"physics.atm-clus"
],
"doi": "10.1140/epjd/e2005-00079-7",
"title": "Importance of electronic self-consistency in the TDDFT based treatment of nonadiabatic molecular dynamics",
"url": "https://arxiv.org/abs/physics/0411104"
},
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